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SCIENCE CHINA Chemistry
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SCIENCE CHINA Chemistry, Volume 62 , Issue 5 : 533-548(2019) https://doi.org/10.1007/s11426-018-9410-0

Recent progress on lithium-ion batteries with high electrochemical performance

Yong Lu , Qiu Zhang , Jun Chen *
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  • ReceivedNov 18, 2018
  • AcceptedDec 21, 2018
  • PublishedFeb 25, 2019
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Abstract

Lithium-ion batteries (LIBs) have been widely used in many fields such as portable electronics and electric vehicles since their successful commercialization in the 1990s. However, the electrochemical performance of current commercial LIBs still needs to be further improved to meet the continuously increasing demands for energy storage applications. Recently, tremendous research efforts have been made in developing next-generation LIBs with enhanced electrochemical performance. In this review, we mainly focus on the recent progress of LIBs with high electrochemical performance from four aspects, including cathode materials, anode materials, electrolyte, and separators. We discuss not only the commercial electrode materials (LiCoO2, LiFePO4, LiMn2O4, LiNixMnyCozO2, LiNixCoyAlzO2, and graphite) but also other promising next-generation materials such as Li-, Mn-rich layered oxides, organic cathode materials, Si, and Li metal. For each type of materials, we highlight their problems and corresponding strategies to enhance their electrochemical performance. Nowadays, one of the key challenges to construct high-performance LIBs is how to develop cathode materials with high capacity and working voltage. This review provides an overview and future perspectives to develop next-generation LIBs with high electrochemical performance.


Funded by

the National Programs for Nano-Key Project(2017YFA0206700)

the National Natural Science Foundation of China(21835004)

and 111 Project from the Ministry of Education of China(B12015)


Acknowledgment

This work was supported by the National Programs for Nano-Key Project (2017YFA0206700), the National Natural Science Foundation of China (21835004), and 111 Project from the Ministry of Education of China (B12015).


Interest statement

The authors declare that they have no conflict of interest.


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    Figure 1

    (a) Schematic illustration and redox mechanism during discharge/charge processes of representative LIBs with LiCoO2 cathode and graphite anode. (b) The global demands and main applications of LIBs in 2016 and 2025 [11]. (c) Cost distributions of different components in LIBs, including cathode, anode, electrolyte, separator, and other materials [11] (color online).

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    Figure 2

    The total production and market shares of different cathode active materials for LIBs in 2016 and 2025 (assumption: Tesla still uses NCA as cathode materials and have a relative success) [11]. LFP: LiFePO4; LCO: LiCoO2; NMC: LiNixMnyCozO2; NCA: LiNixCoyAlzO2; LMO: LiMn2O4 (color online).

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    Figure 3

    Crystal structure of (a) LCO and (b) D-LCO. (c) Charge/discharge curves of D-LCO at C/10 [26]. (d) Cycling and rate performance of D-LCO and P-LCO. (b–d) Reprinted with permission from Ref. [26], copyright 2018, Nature Publishing Group (color online).

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    Figure 4

    (a) Crystal structure of NMC111. (b) The relationship between discharge capacity and thermal stability (as well as capacity retention) of different NMC. (c) The structural illustration and atomic ratio of synthesized FCG NMC. (d) Differential scanning calorimetry curves of the FCG NMC, IC, and OC (all tested at delithiated state). (e) Illustration and corresponding scanning electron microscopy images of LiNi0.7Co0.15Mn0.15O2 sample with pristine state and after exposed to air for 3 months. (f) Schematic diagram of SEI on the surface of LiNi0.7Co0.15Mn0.15O2 cathode. (a) Reprinted with permission from Ref. [30], copyright 2009, Elsevier. (b) Reprinted with permission from Ref. [29], copyright 2013, Elsevier. (c, d) Reprinted with permission from Ref. [35], copyright 2012, Nature Publishing Group. (e) Reprinted with permission from Ref. [38], copyright 2016, The Royal Society of Chemistry. (f) Reprinted with permission from Ref. [41], copyright 2017, Nature Publishing Group (color online).

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    Figure 5

    (a) Crystal structure of layered Li-rich Li2MnO3. (b) Charge/discharge curve evolution of Li1.2Ni0.2Mn0.6O2 (the inset is the corresponding transformation). (c) Cycling performance of pristine Li1.2Ni0.13Co0.13Mn0.54O2 and Sn2+-doped Li1.2Ni0.125Co0.125Mn0.52Sn0.03O2. (d) Schematic diagram for the preparation of LNMO@LBP [55]. The corresponding high-resolution transmission electron microscope (TEM) images of LNMO (e) and LNMO@LBP (f). (g) Rate performance of LNMO and LNMO@LBP (with 0.8 or 1.6 mol% LBP). (b) Reprinted with permission from Ref. [52], copyright 2015, American Chemical Society. (c) Reprinted with permission from Ref. [56], copyright 2017, Science China Press and Springer-Verlag Berlin Heidelberg. (d–g) Reprinted with permission from Ref. [55], copyright 2017, Wiley-VCH (color online).

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    Figure 6

    (a) Crystal structure of olivine LFP. (b) Schematic illustration for the preparation of LFP/rGO composite. (c) Rate performance of LFP/rGO composite. (d) Average discharge capacity of LFP samples with different amounts of Ce coating. (e) Rate performance of G/LFP@C and G/LFP-QDs@C from 0.3 to 200 C. (f) The calculated density of states of pure LFP and Zr, Co co-doped LFP. (b, c) Reprinted with permission from Ref. [66], copyright 2018, Elsevier. (d) Reprinted with permission from Ref. [70], copyright 2014, Elsevier. (e) Reprinted with permission from Ref. [71], copyright 2017, Elsevier. (f) Reprinted with permission from Ref. [64], copyright 2017, Elsevier (color online).

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    Figure 7

    (a) Crystal structure of spinel LMO. (b) Cycling performance of pristine LMO and LMO with different amounts of ZrO2 coating at 55 °C. (c) Initial charge/discharge profiles of LMNO and LMNO with different amounts of Li2SnO3 coating. (b) Reprinted with permission from Ref. [80], copyright 2018, The Royal Society of Chemistry. (c) Reprinted with permission from Ref. [88], copyright 2018, The Royal Society of Chemistry (color online).

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    Figure 8

    (a) The market share of different commercial anode materials in 2016 [11]. (b) Schematic diagram for the preparation of LTO/N-doped C composite. (c) Rate performance of LTO and LTO/N-doped C composite. (b, c) Reprinted with permission from Ref. [100], copyright 2017, Elsevier (color online).

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    Figure 9

    (a) Schematic illustration for the preparation and (b) TEM image of Si@graphene cage composite (the inset of (b) is SAED). (c) Schematic illustration for the preparation of LixSi-Li2O core-shell NPs and their application in Si NPs and graphite. (d) The initial discharge/charge curves and corresponding Coulombic efficiency of MCMB graphite with different amounts of LixSi-Li2O NPs additive. (a, b) Reprinted with permission from Ref. [106], copyright 2018, Wiley-VCH. (c, d) Reprinted with permission from Ref. [110], copyright 2014, Nature Publishing Group (color online).

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    Figure 10

    (a) The formation mechanism of SEI on MoS2 anode without and with 10 wt% FEC additive. (b) Cycling performance of MoS2|NMC523 batteries without and with 10 wt% FEC additive. (c) The insertion behaviour of cations into carbonaceous anode in different electrolytes. Cations (red), anions (green), esters solvent (yellow), non-flammable solvent (blue), salt-derived SEI (green film). (d) Selected discharge/charge profiles of Li-graphite half-cells with concentrated 5.3  mol L−1 LiN(SO2F)2/TMP as electrolyte. (a, b) Reprinted with permission from Ref. [139], copyright 2018, Wiley-VCH. (c, d) Reprinted with permission from Ref. [140], copyright 2017, Nature Publishing Group (color online).

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    Figure 11

    The energy density of different batteries based on Li chemistry (color online).

  • Table 1   Summary on structures, redox mechanisms, working potentials, and theoretical capacities of representative electrode materials for LIBs

    Electrodes

    Materials

    Structure

    (type)

    Redox mechanism

    Potential (V) a)

    Capacity(mA h g–1) b)

    Commercia-lization c)

    Cathode

    LiCoO2

    Layered

    LiCoO2↔CoO2+Li++e−

    3.7

    274

    Y

    LiFePO4

    Olivine

    LiFePO4↔FePO4+Li++e−

    3.45

    170

    Y

    LiMn2O4

    Spinel

    LiMn2O4↔2MnO2+Li++e−

    4.0

    148

    Y

    LiNi1/3Mn1/3Co1/3O2

    Layered

    LiNi1/3Mn1/3Co1/3O2↔Ni1/3Mn1/3Co1/3O2+Li++e−

    3.6

    277

    Y

    LiNi0.80Co0.15Al0.05O2

    Layered

    LiNi0.80Co0.15Al0.05O2↔Ni0.80Co0.15Al0.05O2+Li++e−

    3.6

    278

    Y

    Li1.2Ni0.2Mn0.6O2

    Layered

    Li1.2Ni0.2Mn0.6O2↔Ni0.2Mn0.6O2+1.2Li++1.2e−

    3.5

    378

    N

    LiMn1.5Ni0.5O4

    Spinel

    LiMn1.5Ni0.5O4↔Mn1.5Ni0.5O4+Li++e−

    4.7

    146

    N

    1,4-benzoquinone

    Organic

    C6H4O2+2Li++2e−↔Li2C6H4O2

    2.7

    496

    N

    Anode

    Graphite

    Insertion

    6C+Li++e−↔LiC6

    0.1

    372

    Y

    Li4Ti5O12

    Insertion

    Li4Ti5O12+3Li++3e−↔Li7Ti5O12

    1.55

    175

    Y

    Si

    Alloying

    Si+4.4Li++4.4e−↔Li4.4Si

    0.25

    4212

    Y

    Sn

    Alloying

    Sn+4.4Li++4.4e−↔Li4.4Sn

    0.6

    994

    N

    P

    Alloying

    P+3Li++3e−↔Li3P

    0.5

    2594

    N

    Co3O4

    Conversion

    Co3O4+8Li++8e−↔3Co+4Li2O

    0.9

    890

    N

    Li

    Stripping/plating

    Li↔Li++e−

    0

    3860

    N

    Average discharge voltage (vs. Li+/Li); b) theoretical capacity; c) Y (N) represents the electrode materials have (not) been commercialized nowadays.

  • Table 2   Summary on common salts of electrolyte in LIBs

    Salts

    LiPF6

    LiClO4

    LiBF4

    LiAsF6

    LiN(SO2F)2

    LiN(SO2CF3)2

    H2O sensitivity a)

    Y

    N

    Y

    Y

    Y

    Y

    Al corrosion a)

    N

    N

    N

    N

    Y

    Y

    Ionic conductivity (mS cm–1) b)

    10.0

    9.0

    4.5

    11.1 c)

    10.4 c)

    6.2

    Y and N represents yes and no, respectively; the ionic conductivity of 1 mol L−1 salt dissolved in EC/DMC at b) 20 °C, and c) 25 °C.

  • Table 3   Summary on common solvents of electrolyte in LIBs

    Measured at 25 °C; b) measured at 40 °C; c) measured at 20 °C.

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